Nano Research
·
2023
·
IF 9.9
Liu Guangyong,Lu Yumiao,Lu JunFeng,Wang Yanlei,Liang Shijing,He Hongyan,Jiang Lilong
Electrocatalytic depolymerization of lignin into value-added chemicals offers a promising technique to make biorefining sustainable. Herein, we report a robust trimetallic PdNiBi electrocatalyst for reductive C-O bond cleavage of different lignin model dimers and oxidized lignin under mild conditions. The reduction reaction proceeds with complete substrate conversion and excellent yields toward monomers of phenols (80%–99%) and acetophenones (75%–96%) in the presence of an ionic liquid electrolyte with operational stability. Systematic experimental investigations together with density functional theory (DFT) calculations reveal that the outstanding performance of the catalyst results from the synergistic effect of the metal elements, which facilitates the easier formation of a key C α radical intermediate and the facile desorption of the as-formed products at the electrode. The results open up new opportunities for lignin valorization through the green electrocatalytic approach.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 7
·9032-9043
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IF 2.478
Liu Yunyi,Pan Yongqi,Bai Xudong,Wang Jinchuan,He Caiwang,Xu Zunping,Chen Yi
A conventional ceramic preparation method was used to fabricate the newly designed ternary (K,Na)NbO 3 -based lead-free ceramics, which have the general formula of (0.97- x )K 0.40 Na 0.60 Nb 0.95 Sb 0.05 O 3 –0.03Bi 0.5 K 0.5 HfO 3 – x SrZrO 3 . An X-ray diffraction analysis, together with dielectric-temperature measurements, was performed for determining their phase structures. The crystal structure was found to transition from a rhombohedral-orthogonal phase coexistence to a three-phase coexistence of rhombohedral-orthogonal-tetragonal phases with the increase in SrZrO 3 concentration, and then to a rhombohedral-tetragonal phase coexistence, and finally to a single rhombohedral phase. Near the three-phase coexistence zone, the ceramics exhibit an obviously enhanced electrical activity, with an electromechanical coupling coefficient k p = 0.364 and a piezoelectric constant d 33 = 280 pC/N. Through a microstructure analysis, a slightly excessive amount of SrZrO 3 was found to result in an inhibition for the grain growth of the studied ceramics. These results show that incorporating SrZrO 3 into ternary (K,Na)NbO 3 -based ceramics is still an effective means of constructing phase boundaries and improving the electromechanical properties.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 32
·14724-14738
·
IF 3.591
Lin Qian,Zheng Zeng,Shuyuan Zhang,Kai Xia,Yongfu Guo
In the present work, a poly-o-vanillin-functionalized magnetic nanoparticle of PoVan/CoFe2O4@mSiO2 with core–shell structure was synthesized through a facile, green and low cost method. The rapid removal of Hg(II) by the prepared nanocomposites was researched by batch adsorption experiments and the adsorption conditions were optimized with response surface methodology (RSM). The optimization of RSM shows that the as-prepared PoVan/CoFe2O4@mSiO2 magnetic nanomaterial has a maximal adsorption capability of 263.6 mg g−1 toward Hg(II) ions. The removal process of Hg(II) ions acts in accordance with Langmuir and pseudo-second-order kinetic models. The Dubinin-Radushkevich calculation indicates that the removal process is spontaneous and exothermic. In addition, the adsorption of Hg(II) ions onto PoVan/CoFe2O4@mSiO2 is mainly completed through forming a stable complex by electrostatic attraction and chelation. The adsorption efficiency of the regenerated adsorbent is still high after five cycles. The used adsorbent of PoVan/CoFe2O4@mSiO2 has good magnetic property and can easily be separated from aqueous solution. The results indicate that the magnetic nanomaterial PoVan/CoFe2O4@mSiO2 could be a promising adsorbent to remediate mercury pollution from wastewater.
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2021
·Vol. 105
·期 12
·5147-5158
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IF 4.813
Li Qian,Zhu Xiaoman,Xie Yanli,Zhong Yue
Abstract o -Vanillin is a natural product that has been widely applied in the food and pharmaceutical industries. In this study, we determined that o -vanillin can strongly inhibit the growth of Aspergillus flavus mycelia. However, the inhibition mechanism of o -vanillin is still elusive. The ultrastructural morphology of mycelia was injured, and the cell walls were destroyed. The OH functional groups on cell walls were altered, and the content of protein in mycelial cell walls was reduced by o -vanillin. The content of β-1,3-glucan in cell walls was significantly ( P < 0.05) reduced by o -vanillin in a dose-dependent manner, while chitin was not markedly affected. Moreover, o -vanillin led to an increase in the permeability of cell membranes. o -Vanillin also exhibited a promising antifungal effect on contaminated corn kernels. Therefore, o -vanillin inhibited the growth of mycelia by disrupting the integrity of cell walls and cell membranes. This study not only sheds light on the antifungal mechanism of o -vanillin but also indicates that it is a promising agent for the control of A. flavus infection. Key points o -Vanillin has strong inhibitory effects on A. flavus. o -Vanillin destroyed the integrity of cell walls and cell membranes. o -Vanillin could effectively inhibit the growth of A. flavus on corn kernels.
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Catalysts
·
2020
·Vol. 10
·期 11
·1329
·
IF 3.52
Shijie Hao,Yandi Cai,Chuanzhi Sun,Jingfang Sun,Changjin Tang,Lin Dong
Monolithic Mn-Fe-Ce-Al-O catalyst with honeycomb cordierite ceramic as a carrier was reported for the first time for low temperature deNOxapplication. In the reaction of selective catalytic reduction (SCR) of NO with NH3, a NO conversion of above 80% at 100 °C was obtained. Notably, the catalyst also showed excellent resistance against SO2and H2O. About 60% NO conversion was maintained after successive operation in the mixed stream of SO2and H2O for 168 h. The Brunner−Emmet−Teller (BET) measurement, SEM, EDS, thermogravimetric analysis (TG), FT-IR, and XPS results of the used catalysts indicated that certain amounts of ammonium sulfate was formed on the surface of the catalyst. XPS results revealed that partial of Fe2+was oxidized to Fe3+during the reaction process, and Fe2+species have strong redox ability, which can explain the decrease in activity after reaction. In addition, SO2and H2O induced a transformation of Ce from Ce4+to Ce3+on the surface of the catalyst, which increased the amount of chemisorbed oxygen. Owing to these factors, the addition of Ce and Fe species contributes to excellent resistance of the catalyst to SO2and H2O.Keywords:honeycomb catalyst;Mn-Fe-Ce-Al-O;low temperature denitration;water and sulfur resistance
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 9
·1-11
·
IF 6.232
Ye Mingshu,Lin Bixia,Yu Ying,Li He,Wang Yumin,Zhang Li,Cao Yujuan,Guo Manli
By using graphene quantum dots (GQDs) and o -phenylenediamine (OPD), a ratiometric fluorescence probe was designed for the highly sensitive and selective detection of AChE. GQDs with strong fluorescence were synthesized by the one-step hydrothermal method. The optimal emission wavelength of GQDs was 450 nm at the excitation wavelength of 375 nm. MnO 2 nanosheets with a wide absorption band of 300–600 nm were prepared at room temperature. Because of the extensive overlap between the absorption spectrum of MnO 2 nanosheets and the excitation and emission spectra of GQDs, the fluorescence of GQDs at 450 nm was efficiently quenched by the inner-filter effect. Meanwhile, due to the peroxidase-like activity of MnO 2 nanosheets, OPD was catalytically oxidized to 2,3-diaminophenazine (oxOPD), a yellow fluorescent substance with a new emission peak at 572 nm. When AChE was present, the substrate acetylthiocholine (ATCh) was hydrolyzed to thiocholine (TCh) that is capable of decomposing MnO 2 nanosheets. Therefore, the quench of GQDs and the oxidation of OPD by MnO 2 nanosheets were suppressed, resulting in the fluorescence recovery of GQDs at 450 nm, while the fluorescence decrease of oxOPD at 572 nm. Utilizing the fluorescence intensity ratio F 450 /F 572 as the signal readout, the ratiometric fluorescence method was established to detect AChE activity. The ratio F 450 /F 572 against the AChE concentration demonstrated two linear relationships in the range 0.1–2.0 and 2.0–4.5 mU mL −1 with a detection limit of 0.09 mU mL −1 . The method was applied to the detection of positive human serum samples and the analysis of the inhibitor neostigmine. Due to the advantages of high sensitivity, favorable selectivity, and strong anti-interference, the method possesses an application prospect in clinical diagnosis of AChE and the screening of inhibitors.
Schematic presentation of a ratiometric fluorescence method for the detection of acetylcholinesterase (AChE). The fluorescence of graphene quantum dots (GQDs) is quenched and o -phenylenediamine (OPD) is oxidized to generate fluorescent product 2,3-diaminophenazine (oxOPD) by MnO 2 nanosheets. When AChE is present, acetylthiocholine iodide (ATCh) is hydrolyzed to thiocholine (TCh) with reducibility for decomposing MnO 2 nanosheets. Due to the decomposition of MnO 2 nanosheets, the quenching of GQDs and oxidation of OPD are suppressed. The fluorescence of GQDs at 450 nm is enhanced, while the fluorescence of oxOPD at 572 nm is reduced. The fluorescence intensity ratio F 450 /F 572 is used to establish the ratiometric fluorescence method for AChE activity.
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TALANTA
·
2020
·
IF 5.339
Nan Yin,Ruihuan Zhao,Jie Zhang,Dingding Yang,Zhimin Guo,Rui Liu,Xin Yao
Abnormal O-linked N-acetylglucosamine (O-GlcNAc) concentrations have been associated with many diseases, but the lack of accurate detection method limited O-GlcNAc to be used as a biomarker in clinical diagnosis. Then O-GlcNAc transferase (OGT) has drawn researchers’ attention as it closed related to the level of O-GlcNAc and be considered to be a promising new target for diseases diagnosis. Nevertheless, the existing OGT detection methods are either need labeling or the sensitity can not meet the needs of clinic testing. Herein, a label-free and sensitive SPR biosensor was developed for accurate detection of OGT based on a multi-functional peptide. The designed peptide contains three recognition sites, one is the cleavage site of protease K, one is the O-GlcNAcylated site by OGT, and another is six histidine which be used as the signal report probe to recognize Ni 2+ . The immobilized peptide would be cleavaged by proteinase K, then the His-tag residue part will leave the surface of Au film, resulting less His-tag could bind to Ni 2+ and a small SPR signal would be record. If the peptide is O-GlcNAcylated by OGT, the cleaving reaction would be limited due to the adjacent site of O-GlcNAcylation. Then more His-tag can be left on the Au film and a bigger SPR signal could be record, this signal is associated with the concentration of OGT. Utilizing the change of the peptide configuration as a signal report probe for OGT detection not only avoids labeling of peptide, but also makes the method more sensitive. The determination linear range of OGT is from 2.00 × 10 −13 to 5.00 × 10 −8 M with a detection limit of 1.19 × 10 −13 M, and the separation of two enzyme reactions ensured the high selectivity of the method. Finally, the sensing system was successfully used for OGT detection in blood samples with satisfied recovery. In summary, the label-free SPR platform for accurate detection of OGT in real samples is helpful to promote OGT serve as a biomarker for early clinical diagnosis of O-GlcNAc related diseases.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Hairus Abdullah,Noto Susanto Gultom,Hardy Shuwanto,Worku Lakew Kebede,Dong-Hau Kuo
Zn(O,S) has been successfully doped with different amounts of Ho and characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), and transient photocurrent (TPC). The as-prepared Ho-doped Zn(O,S) catalysts with different Ho amounts are evaluated for hydrogen evolution reaction. The catalyst with the best performance in evolving hydrogen is further utilized to hydrogenate 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). It is found that doping with Ho obviously enhanced charge transfer and photoresponse properties of the catalyst. Therefore, the modified Zn(O,S) can optimally evolve hydrogen by 18 624 μmol/g, which is 20% higher than that of pristine Zn(O,S). Subsequently, the in situ generated hydrogen ions on catalyst surfaces also play an important role as a hydrogen source to hydrogenate 4-NP to 4-AP without any reducing agents such as NaBH4, which is commonly used as a hydrogen source. As Ho is doped in the lattices of Zn(O,S), it acts not only to separate photocarriers and to enhance the charge transfer but also to shorten the diffusion time of nitrophenolate ions to catalyst surfaces for further photocatalytic hydrogenation reaction (PHR) process. A plausible PHR mechanism has been provided to elucidate the great performance of Ho-modified Zn(O,S) for photocatalytic hydrogenation.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 45
·期 1
·365-372
·
IF 3.288
Yancong Li,Jiliang Ma,Zhendong Liu,Dongnv Jin,Gaojie Jiao,Yanzhu Guo,Qiang Wang,Jinghui Zhou,Runcang Sun
A simple and efficient photocatalytic method for the synthesis of dihydropyrimidinones (DHPMs) and their derivatives via porous ultrathin carbon nitride nanosheets (p-CNNs) without solvents was demonstrated. The yields of 3,4-dihydropyrimidin-2(1H)-ones/thiones and their derivatives were up to 97.0%. Furthermore, the yield of 5-ethoxycarbonyl-6-methyl-4-phenyl-3,4-dihydropyrimidin-2(1H)-one in the 10th cycle retained 98.9% of its 1st value. Considering the environmental and economic benefits, this work exhibits various merits including excellent yields, environmental friendliness, inexpensiveness, and avoiding the use of solvents and metal-based photocatalysts. In addition, the excellent performance of the p-CNNs and environmentally benign reaction system have also been checked by the photocatalytic synthesis of 12-phenyl-9,9-dimethyl-8,9,10,12-tetrahydrobenzo[a]xanthen-11-one and 5-phenyl-1(4-methoxyphenyl)-3[(4-methoxy-phenyl)-aminol]-1H-pyrrol-2(5H)-one. This work paves a new way for carrying out a three-component reaction using metal-free photocatalysts under mild reaction conditions.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 5
·1-9
·
IF 6.232
Mathivanan Dhamodiran,Tammina Sai Kumar,Wang Xiuli,Yang Yaling
A selective and sensitive fluorescent technique is proposed to determine o -phenylenediamine (OPD) and hydrogen peroxide (H 2 O 2 ). This is carried out by utilizing enzyme mimics carbon dots (N/Cl-CDs) and fluorescent probe carbon dots (N/Zn-CDs). The synthesized N/Cl-CDs and N/Zn-CDs were characterized by transmission electron microscopy (TEM), X-ray powder diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and Ultraviolet-visible spectrophotometry techniques. The particle size of synthesized carbon dots was found to be 4.1 ± 1.09 nm and 3.3 ± 1.82 nm for N/Cl-CDs and N/Zn-CDs, respectively. The N/Cl-CDs showed a noticeable intrinsic peroxidase-like activity, which could catalyze the oxidization of OPD by H 2 O 2 to form the yellow colored product 2,3-diaminophenazine (DAP). The N/Zn-CD fluorescence was quenched directly by DAP through the inner filter effect (IFE). As a result, a novel double carbon dot system as enzyme mimics and fluorescent investigations to recognize OPD and H 2 O 2 was obtained. The N/Cl-CDs were synthesized by deep eutectic solvent (DES) source and chamber electric furnace. N/Zn-CDs were also synthesized with the quantum yield of 27.52% through the tubular furnace technique using ethylenediamine tetra acetic acid disodium zinc salt and ascorbic acid as precursors. The detection limits were found to be 0.58 μM and 0.27 μM for OPD and H 2 O 2 , respectively. The nanoprobe was applied to real sample analysis, which showed excellent recovery in the range of 95.8–103.5% and 98.6–107.3% for OPD and H 2 O 2, respectively. The dual emission carbon dots as enzyme mimic and fluorescent probe sensing system opens a new platform for determination of H 2 O 2 and OPD in real samples.
Schematic illustration of the preparation of double carbon dots and determination process of o -phenylenediamine (OPD) and hydrogen peroxide (H 2 O 2 )
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Naixu Li,Xu Liu,Jiancheng Zhou,Quanhong Ma,Maochang Liu,Wenshuai Chen
Direct conversion of cellulose into ethylene glycol is a promising route for transforming sustainable biomass resources into high-value chemicals. Although numerous attempts have been made to exploit tungsten-based hydrogenolysis catalysts in the catalytic conversion of cellulose to ethylene glycol for high conversion rate and selectivity, maintaining catalyst stability remains challenging. Herein, we have developed a Ni–W/M catalyst with good catalytic performance and stability, which were obtained by calcining Ni–W/MIL-125(Ti) precursor. The synthesized catalyst showed good cellulose conversion rate (100%) and ethylene glycol yield (68.7%). The tungsten species was linked to the TiO2 support by Ti–O–W bonds to reduce loss of the active tungsten component. The formation of new bonds enhanced the catalyst stability and durability, enabling the catalysts to retain high catalytic activity during recycling.
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JOURNAL OF CHROMATOGRAPHY A
·
2020
·
IF 4.049
Jianli Han,Qinghui Chen,Wanjun Jin,Meiyi Zou,Yu Lu,Yuxia Liu,Chengjian Wang,Zhongfu Wang,Linjuan Huang
Mass spectrum (MS) is one of the most commonly used tools for qualitative and quantitative analysis of glycans. However, due to the complexity of biological samples and the low ionization efficiency of glycans, these need to be purified and derivatized prior to MS analysis. Existing purification strategies require a combination of multiple methods and are cumbersome to operate. Here, we propose a new method for the purification of glycoprotein N/O-glycans and their derivatives using a hand-packed absorbent cotton hydrophilic interaction chromatography column (HILIC). The method's reliability and applicability were verified by purifying N/O-glycans and the derivatives of standard glycoproteins, such as chicken albumin and porcine stomach mucin. Stable isotope labelling was used to compare the glycans’ recovery following different purification methods. Absorbent cotton HILIC was also successfully applied for the analysis of human serum and fetal bovine serum glycoprotein N-glycans. Finally, testing revealed high binding capacity (9 mg/g −1 maltohexaose/absorbent cotton) and good recovery (average recovery was 91.7%) of glycans. Compared with traditional procedures, the proposed purification method offers considerable advantages, such as simplicity, high efficiency, economy, universality, and broad applicability for the pretreatment of glycans and their derivatives in biological samples prior to MS analysis.
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